May 1, 2024
Journal Article

Tailoring solvation solvent in localized high-concentration electrolytes for lithium||sulfurized polyacrylonitrile batteries

Abstract

Sulfurized polyacrylonitrile (SPAN) is a promising cathode material for lithium-sulfur (Li-S) batteries due to its significantly reduced polysulfide (PS) dissolution compared to the elemental S cathode. Although conventional carbonate-based electrolytes is stable with SPAN electrodes, it is less stable with Li metal anode (LMA). Recently, localized high-concentration electrolytes (LHCEs) have been developed to improve the stability of LMA. Here, we report a new strategy to further improve the performance of LI||SPAN batteries by replacing the conventional solvating solvent 1,2-dimethoxyethane (DME) in the LHCE with a new solvating solvent, 1,2-diethoxyethane (DEE), the new LHCEs exhibits less reactivity against Li2S2, alleviates PS dissolution, forms a better cathode-electrolyte interphase layer on the SPAN, and enhances structure reversibility even at elevated temperature (ET, 45°C). With the same salt and diluent as in other LHCEs, the LHCE with DEE leads to better performance in Li||SPAN batteries (with 82.9% capacity retention after 300 cycles at ET), preservation of SPAN cathode structure, and suppression of the volume change of LMA. The similar strategy on tailoring the solvating solvents in LHCEs can also be used in other rechargeable batteries to improve their performances.

Published: May 1, 2024

Citation

Kim J., P. Gao, Q. Miao, Q. Zhao, M.M. Rahman, P. Chen, and X. Zhang, et al. 2024. Tailoring solvation solvent in localized high-concentration electrolytes for lithium||sulfurized polyacrylonitrile batteries. ACS Applied Materials & Interfaces 16, no. 16:20618-20625. PNNL-SA-193968. doi:10.1021/acsami.4c02326